Closed system generation and containerization of radioisotopes for eluting a daughter radioisotope from a parent radioisotope

ABSTRACT

Apparatus for eluting a sterile daughter radioisotope from a parent radioisotope and containerizing the resultant eluate in an evacuated container having a rubber stopper, providing for delivery of a sterile pyrogen-free eluant from a sealed supply through a sterile charge of the parent radioisotope sealed in a shielded generator and thence to a tubular needle adapted to be pierced through the stopper of the evacuated container for suctioning the eluant from the sealed eluant supply into the generator and for suctioning the resultant eluate into the container. The needle is applied to a fitting on a plunger adapted to be pushed down to pierce the needle through the stopper. Eluate is delivered from the generator to the fitting for flow through the needle via an eluate conduit having a flexible tubing portion permitting movement of the plunger and the fitting, with an arrangement whereby the plunger, when retracted, pinches the flexible tubing portion closed, the flexible tubing portion being automatically released when the plunger is driven downward to open the flexible tubing portion for flow therethrough of the eluate under suction induced by the piercing of the needle through the stopper into the evacuated container.

United States Patent Montgomery et al.

[15] 3,655,981 [451 Apr. 11, 1972 [54] CLOSED SYSTEM GENERATION AND CONTAINERIZATION OF RADIOISOTOPES FOR ELUTING A DAUGHTER RADIOISOTOPE FROM A PARENT RADIOISOTOPE 72] Inventors: James R. Montgomery, Maplewood; Lloyd G. Struttman, St. Louis, both of Mo.

Primary Examiner--James W. Lawrence Assistant Examiner-Morton J. F rome Attorney-Keenig, Senninger, Powers and Leavitt [57] ABSTRACT Apparatus for eluting a sterile daughter radioisotope from a parent radioisotope and containerizing the resultant eluate in an evacuated container having a rubber stopper, providing for delivery of a sterile pyrogen-free eluant from a sealed supply through a sterile charge of the parent radioisotope sealed in a shielded generator and thence to a tubular needle adapted to be pierced through the stopper of the evacuated container for suctioning the eluant from the sealed eluant supply into the generator and for suctioning the resultant eluate into the container. The needle is applied to a fitting on a plunger adapted to be pushed down to pierce the needle through the stopper. Eluate is delivered from the generator to the fitting for flow through the needle via an eluate conduit having a flexible tubing portion permitting movement of the plunger and the fitting, with an arrangement whereby the plunger, when retracted, pinches the flexible tubing portion closed, the flexible tubing portion being automatically released when the plunger is driven downward to open the flexible tubing portion for flow therethrough of the eluate under suction induced by the piercing of the needle through the stopper into the evacuated container.

31 Claims, 8 Drawing Figures Patented April 11, 1972 4 Sheets-Sheet 2 Patented April 11, 1972 4 Sheets-Sheet 5 Patented A ril 11, 1972 4 Sheets-Sheet 4 w Ann vlarlrllltl l wln i CLOSED SYSTEM GENERATION AND CONTAINERIZATION OF RADIOISOTOPES FOR ELUTING A DAUGHTER RADIOISOTOPE FROM A PARENT RADIOISOTOIPE BACKGROUND OF THE INVENTION This invention relates to the generation and containerization of radioactive isotope solutions, and more particularly to apparatus for the generation and containerization under sterile conditions of such solutions obtained as the eluate in a closed system radioisotope generator.

The invention is particularly concerned with the preparation and packaging, in a sterile closed system, of a solution of a daughter radioisotope, such as technetium-99m, generated from a parent radioisotope, such as molybdenum-99. Conventionally, the preparation of a daughter radioisotope from a parent radioisotope has been carried out using a generator containing the parent radioisotope and an anion exchange medium or other medium, such as alumina, having a high adsorptive capacity for the parent radioisotope but a low adsorptive capacity for the daughter radioisotope. The desired daughter radioisotope is eluted by washing with a suitable solvent or eluant such as a sterile, pyrogen-free isotonic saline solution. The resulting eluate containing the daughter radioisotope in the form of a dissolved salt is useful as a diagnostic agent, for example, and is adapted for intravenous administration.

The generator containing the parent radioisotope adsorption medium for eluting the daughter radioisotope is frequently referred to in the art as a cow, and the elution of the daughter radioisotope therefrom is generally referred to in the art as milking the cow."

Some widely used daughter radioisotopes used in medical diagnosis have relatively short half-lives, e.g., 6 hours, and it is important therefore that they be generated or prepared shortly before usage in the hospital, clinic or other place of use. Thus, there is need, for example, for apparatus enabling generation and containerization under sterile conditions once a day in a hospital or clinic of the eluate, also under conditions wherein the user of the apparatus is afforded maximum protection against radioactive emission from the generator. Prior apparatus for the purpose, such as disclosed in US. Pat. Nos. 2,942,943 and 3,369,121 and in the copending coassigned US. patent application of Donald J. Shumate, Ser. No. 658,872, filed Aug. 7, I967, titled Closed System Generation and Containerization of Radioisotopes, issued as US. Pat. No. 3,535,085, Oct. 20, 1970, has not been wholly satisfactory, primarily on account of the necessity for carrying out a number of hand operations while the shield for the generator is open, thus exposing the hands and possibly other parts of the operator to radiation. Since the decay characteristics of most of the parent-daughter radioisotope combinations presently in large-scale use require that the generator (the cow) be milked" daily, the use of the above prior devices undesirably involves daily exposure of the operator to radioactivity during the milking operation.

SUMMARY OF THE INVENTION Accordingly, among the several objects of this invention may be noted the provision of an improved closed system radioisotope generation and containerization apparatus, for the generation and containerization of a sterile solution of a daughter radioisotope, which satisfies radiation safety requirements; the provision of such an apparatus which minimizes operator handling and exposure; and the provision of such an apparatus which is easy and economical to use.

In general, apparatus of this invention is adapted for eluting a daughter radioisotope from a parent radioisotope and for containerizing the resultant eluate in an evacuated container having a closure adapted to be pierced by a needle. It comprises a generator containing a supply of the parent radioisotope, a shield enclosing the generator for shielding the user against radioactive emission from the generator, means for holding a supply of eluant adjacent the shield and generator, and an eluant conduit extending from the eluant supply means through the shield and into the generator. A tubular fitting adapted for attachment thereto at one end of a tubular needle for piercing said closure is mounted adjacent the shield and generator for movement away from a retracted position in the direction of length of the needle to cause the needle to pierce said closure. An eluate conduit extends from the generator through the shield and has a flexible tubing portion connected to the other end of the tubular fitting permitting movement of said fitting. The eluant conduit, generator, eluate conduit and fitting constitute a closed passage from the eluant supply to the needle. Associated with said fitting is means for effecting closure of said eluate conduit when said fitting is in its said retracted position and opening of said eluate conduit when said fitting is moved to cause the needle to pierce the closure of said evacuated container for flow of eluant from the eluant supply means through the eluant conduit into the generator for eluting the daughter radioisotope from the parent radioisotope in the generator and flow of the resultant eluate from the generator through the eluate conduit, fitting and needle into the evacuated container. Other objects and features will be in part apparent and in part pointed out hereinafter.

BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a perspective of an apparatus made in accordance with this invention, a plastic case of the apparatus being illustrated as transparent for viewing interior detail;

FIG. 2 is a plan of the FIG. 1 apparatus;

FIG. 3 is a view in elevation of the apparatus, showing a container in position for receiving the eluate eluted from a generator in the case;

FIG. 4 is a vertical section on line 4-4 of FIG. 2;

FIG. 5 is a vertical section on line 55 of FIG. 2;

FIG. 6 is a horizontal section on line 6-6 of FIG. 3;

FIG. 7 is an enlarged fragment of FIG. 4 showing a plunger and tubular needle of the apparatus driven downward with the needle pierced through the stopper of the container; and

FIG. 8 is an enlarged vertical section of a generator or cow" of the apparatus.

Corresponding reference characters indicate corresponding parts throughout the several views of the drawings.

DESCRIPTION OF THE PREFERRED EMBODIMENT Referring to the drawings, apparatus made in accordance with this invention is shown essentially to comprise a generator or cow 1 containing a sterile pyrogen-free supply 3 of a parent radioisotope. The generator is enclosed in a shield 5 for shielding the user of the apparatus against radioactive emission from the generator. At '7 is indicated means for holding a sterile pyrogen-free supply of an eluant with the eluant under atmospheric pressure. An eluant conduit 9 extends from means 7 through the shield and into the generator.

At 11 is indicated a tubular fitting adapted for attachment thereto at one end (its lower end) of a tubular needle 13, which may be a conventional hypodermic needle. The apparatus, as will appear, provides for the sealed sterile containerization of a sterile pyrogen-free eluate eluted from the parent radioisotope in a sealed sterile evacuated container or vial 15, shown as comprising a glass bottle having a neck 17 sealed at its upper end by a closure 19 adapted to be pierced by the needle 13. Closure 19 may be a conventional rubber stopper, and is shown as having an aluminum foil cover 21. This cover has a removable circular central section, shown removed in FIGS. 1 and 7 leaving an opening 23 in the cover.

Means generally designated 25 is provided for mounting the tubular fitting 11 (and needle 13) for movement away from the retracted position of FIG. 3 in the direction of length of the needle to cause the needle to pierce the closure or stopper 19. An eluate conduit 27 extends from the generator through the shield and has a flexible tubing portion 29 connected to the other end (the upper end) of the tubular fitting 11 permitting the stated movement of the fitting. At 31 is indicated means associated with the fitting 11 for effecting closure of the eluate conduit when the fitting is in its retracted position and opening of the eluate conduit when the fitting is moved downward to cause the needle 13 to pierce the stopper 19 of the evacuated container 15, with resultant suctioning of eluant from the eluant supply means 7 into the generator 1 for eluting a daughter radioisotope from the parent radioisotope in the generator and suctioning of the resultant eluate from the generator through the eluate conduit 27, fitting l1 and needle 13 into the evacuated container 15.

The generator 1, as shown, comprises an elongate cylindric vessel 33 constituted by a glass tube resembling a test tube having a convergent closed lower end 35 of hemispherical form and a neck 37 at its upper end. A pierceable closure constituted by a rubber stopper 39 is plugged in the neck to seal the vessel. This has an aluminum foil cover 41 from which a circular central section has been removed. A fritted glass filter 43 is mounted in the vessel just above its hemispherical lower end. The vessel 33 is necked down as indicated at 45, and the filter is lodged in the necked-down portion and bonded therein. The space below the filter constitutes an eluate chamber 49, and the filter serves as means for maintaining the supply 3 of the parent radioisotope spaced from the lower end of the vessel, so that chamber 19 is maintained free of the supply 3.

The filter 43 has a center hole 51. The eluate conduit 27 comprises a length of relatively small diameter metal tubing 53 (e.g., stainless steel tubing) bent to have a vertical leg 55 and a horizontal arm 57. The lower end of the vertical leg 55 is beveled as indicated at 59. The vertical leg 55 extends down through the stopper 39, its beveled lower end 59 permitting it to be pierced through the stopper, and reaches down through the center hole 51 in the filter 43 substantially to the bottom of the hemispherical lower end 35 of the vessel 33. The hole 51 may be of substantially larger diameter than the leg, and the latter may be sealed in the hole by a suitable sealant, such as silicone rubber as indicated at 61.

The supply or charge 3 of the parent radioisotope is packed in the vessel above the filter and surrounds the vertical leg 55 of the tubing 53, which leg extends down generally centrally of the vessel. The charge 3 comprises the parent radioisotope adsorbed on an anion exchange medium, alumina or other suitable medium, in granular form, and having under suitable conditions, a high adsorption capacity or affinity for the parent radioisotope but a low adsorption capacity for the daughter radioisotope. For generation of technetium-99m, for example, the charge 3 in the vessel may comprise molybdenum-99, in the form of ammonium molybdate, as the parent radioisotope, adsorbed on alumina, the latter constituting a medium having a high adsorption capacity for ammonium molybdate Mo-99 but a low adsorption capacity for the daughter technetium- 99m compound in the presence of certain known eluting solutions.

The eluant conduit 9 comprises a length of relatively small diameter metal tubing 63 (e.g., stainless steel tubing) like tubing 53, bent to have a relatively short vertical leg 65 and a horizontal arm 67. The lower end of the vertical leg is beveled as indicated at 69. The vertical leg 65 extends down through the stopper 39, its beveled lower end 69 permitting it to be pierced through the stopper, and terminates just below the stopper. The charge 3 substantially fills the vessel from filter 43 up to the stopper, and leg 65 may reach down just into the top of the charge. The eluant conduit 9 further comprises a length of flexible tubing 71 interconnecting the eluant supply means 7 and a fitting 73 on the end of the arm 67 of tubing 03. As herein shown, the eluant supply means 7 comprises a plastic bag or transfer pack containing the eluant, this bag being subject to being squeezed by atmospheric pressure, the bag having an outlet 75 from which flexible tubing 71 extends to the fitting 73 on the end of arm 67. The eluant may be, for example, a sterile pyrogen-free saline solution which in the case of elution of technetium-99m as the daughter radioisotope from molybdenum-99, results in the daughter radioisotope being present in the eluate as sodium pertechnetate.

As herein illustrated, the shield 5 for the generator comprises a relatively thick-walled receptacle, which may be made of lead or other suitable shielding material, formed to provide a cylindric chamber 77 extending down from the top of the receptacle, and formed with supporting legs 79. Chamber 77 has a diameter somewhat greater than that of the generator 1 and a length (height) somewhat greater than that of the generator. The receptacle is formed with two diametrically opposite slots 81 extending down from its upper end, and is closed,'after insertion of the generator therein, by a closure constituted by a plug 83 made of lead or other suitable shielding material inserted in the upper end of the chamber. The generator is inserted in the chamber with arms 57 and 57 of the metal tubing portions 53 and 63 of the eluant and eluate conduits 9 and 27 extending laterally outward through the slots 81 at the lower ends of these slots (the generator, in effect, being hung in the chamber by engagement of arms 57 and 67 with the lower ends of the slots). The plug has two ears 85 extending outward therefrom diametrically opposite one another fitting in the slots and bearing on the arms. The plug may be removably secured to the receptacle (after insertion of the generator) as by adhesive tape (not shown) or in any other suitable manner.

The shield 5 with the generator 1 sealed therein and the plastic bag 7 containing the eluant are supplied in a case generally designated 87. This case, which may be made of either transparent or opaque plastic or any other suitable material, comprises a bottom section 89 and a cover 91. The bottom section 89 has a circular flat bottom plate 93, an internal cylindric wall 95 extending up from bottom 93 and concentric therewith, and an external peripheral wall 97 extending up from the margin of bottom 93. Wall 97 is part cylindric, having a gap 99 therein spanning somewhat less than of arc. Radial partitions 101 and 103 extend from the internal wall to the peripheral wall 97, the outer ends of these partitions (which lie in planes at right angles to one another) being joined to the peripheral wall 97 on opposite sides of the gap 99. Partitions 105 and 107 extend from the internal wall 95 to the peripheral wall 97 diametrically opposite partitions 101 and 103. A curved panel 109, convexly curved as viewed from outside the case, extends between the vertical margins of the peripheral wall 97 on opposite sides of the gap 99 in wall 97 and butts against the internal wall 95. This curved panel defines a recess 111 opening inward from the respective side of the case, bottomed by portion 93a of the bottom plate.

The walls 95 and 97 and partitions 101, 103, 105, and 107 are of equal height, somewhat less than the height of the shield 5. The curved panel 109 has an upward extension 113 of reduced width extending up above the level of the top of walls 95 and 97 and the partitions. The top of the recess 111 is closed by a horizontal head plate 115 at the top of extension 113, this plate 115 having an inner edge curved in correspondence with the curvature of the panel, and an outer edge 117 curved on an are centered in the vertical central axis of the case bottom section 89 of radius corresponding to the radius of the inside of the peripheral wall 97. Plate 115 has a centrally located vertical opening 119 and an annular boss 121 extending upward around this opening.

The internal wall 95 has an internal diameter somewhat larger than the cross section of shield 5 and defines a chamber 123 located centrally of the case bottom section 89 receiving the shield. The feet of the latter are confined within a centering ring 125 projecting up from bottom 93 of section 09 within the wall 95. Partitions 105 and 107 in conjunction with walls 95 and 97 define a compartment 127 receiving the plastic eluant bag 7.

The cover 91 comprises a cylindric external peripheral wall 129 having the same diameter as wall 97, and a cylindric internal wall 131 having the same diameter as wall 95. Radial partitions 133, 135, 137, and 139 (corresponding to partitions 101, 103, 105, and 107) extend between these walls. The upper rims of walls 129 and 131 are at the same level, but wall 129 extends down somewhat farther than wall 131. Wall 129 has a relatively wide shallow notch 141 in its lower margin, the width of this notch corresponding to the width of gap 99. Extending around the inside of wall 129 at the lower end thereof from adjacent one side of the notch to the other is a rim 143 which projects down below the lower edge of wall 129 and which has a telescopic sliding fit within wall 97 of the case bottom section 89. The downwardly projecting portion of this rim has notches 145 receiving the partitions 103, 105, 107, and 109. Wall 131 defines a chamber 146 for the upper end of shield 5, and has notches 147 at its lower end for passage of arms 57 and 67. Chamber 146 is closed at the top by a circular top plate 149 spaced somewhat below the upper end of wall 131 to provide a circular compartment 151 for holding a supply of needles 13. A plate 153 closes the top of the space bounded by partitions 133 and 135 and walls 129 and 131, and a plate 155 closes the top of the space bounded by partitions 137 and 139 and walls 129 and 131, defining oppositely located downwardly opening chambers 157 and 159. Plates 161 close the bottom of the space bounded by partitions 133 and 139 and the bottom of the space bounded by partitions 135 and 137 and walls 129 and 131, defining two oppositely located upwardly opening compartments 163 for holding a supply of evacuated bottles 15.

The means 25 for mounting the tubular fitting 11 includes a tubular plunger 165 mounted for vertical sliding movement in the opening 119 in the plate 115 and in an aligned opening 167 in the plate 153 of the cover, these plates constituting a portion of the case 87 overhanging the recess 111. An annular boss 169 extends down from plate 153 around the opening 167, and has an annular groove 171 of inverted V-section in its lower end. The plunger has a plug 173 in its lower end, the fitting 11 being received in an axial opening 175 in the plug. The fitting extends down from the plug for attachment of the needle 13 to the lower end of the fitting with the needle ex tending downward from the lower end of the fitting by applying a ferrule 177 on the upper end of the needle to the lower end of the fitting. The plunger has a lateral opening 179 (see FIG. 7) spaced from its lower end located between the plates 115 and 153. The flexible tubing portion 29 of the eluate conduit 27 extends through this opening and down through the plunger to a connection at 181 with the upper end of fitting 1 1. The plunger has an annular collar 183 thereon immediately below the opening 179 formed with an upwardly extending annular rib 185 of inverted V-section matching the V-section groove 171 in boss 169. A coil compression spring 187 surrounding the plunger reacts from the boss 121 against the collar 183 to bias the plunger upward toward its raised retracted position in which it is illustrated in FIG. 4. A knob 189 is provided at the upper end of the plunger. Axially extending keys 191 on the plunger slide in keyways 193 at opposite sides of opening 167 to prevent rotation of the plunger about its vertical axis.

The collar 183 on the plunger 165 constitutes a movable jaw member which functions in conjunction with boss 169 as a fixed jaw member to pinch closed the flexible tubing portion 29 of the eluate conduit where it extends into the opening 179 when the plunger is biased upward to its raised retracted position by the spring 187 (see FIGS. 1, 3, and 4). The latter exerts sufficient upward force on the plunger for this purpose. When the plunger is driven downward against the return bias of spring 187, the pinch on the tubing portion 29 is released and the eluate conduit is thus opened for flow of eluate.

The generator 1, containing the sterile pyrogen-free supply 3 of the parent radioisotope, and itself being made sterile and pyrogen-free (as by heating) is placed in chamber 77 in the lead shield 5, and the latter is closed by the plug 83. The shield 5 and the plastic bag 7 containing the supply of sterile pyrogen-free eluant are placed in the bottom section 89 of the case 87, tubing 71 is connected to fitting 73, and tubing 29,

extending from fitting 11 out of the plunger through opening 179, is connected to a fitting 195 on the end of arm 57. The metal tubing and flexible tubing portions of the eluant and eluate conduits and fitting 11 are all in sterile and pyrogenfree condition, and it will be understood that the needles 13 are supplied in sterile pyrogen-free condition. The cover 91 of the case 87 is applied to the bottom section 89, and secured thereto in any suitable manner, as by adhesive tape, or by use of a solvent for the plastic of the case and cover to cause them to become bonded together. The containers or vials 15, as initially supplied, are sterile and pyrogen-free and evacuated of air. They may have graduations marked thereon for indicating volume of eluate drawn thereinto.

In the use of the apparatus, an evacuated container or vial 15, held in a lead cup 197, is placed in the recess 111 of the case 87 with the stopper 19 of the vial in line with the needle 13 on the lower end of the fitting l 1. The plunger 165 is then manually pushed downward against the upward return bias of spring 187 to cause the needle 13 to pierce through the stopper 19 of the vial (see FIG. 7) and simultaneously to effect release of the flexible tubing portion 29 of the eluate conduit 27 by the jaw member 183 so as to open the eluate conduit. This results in suctioning of the eluant from the eluant supply bag 7 (which is under atmospheric pressure) through the eluant conduit 9 into the generator 1 for eluting the daughter radioisotope from the parent radioisotope in the generator. The resultant eluate passes down through the filter 43 into the eluate chamber 49 at the lower end of the generator, and is suctioned upward through leg 55 of metal tubing 53 and thence through flexible tubing portion 29 of the eluate conduit 27, and fitting 11 and needle 13 into the evacuated vial 15. The plunger 165 is held down until the desired amount of eluate has been suctioned into the vial, and then released to be returned to its raised retracted position by the spring 187, resulting in pinching of the flexible tubing portion 29 of the eluate conduit 27 to cut off further flow as might otherwise occur due to siphoning action. The filled vial is then taken away for ultimate use, and the apparatus is ready for the next milking" operation.

It will be observed that the milking operation is carried out without opening of the shield 5, hence does not involve any exposure of the operator to radiation from the generator 1. The latter at all times remains essentially sealed within the shield, which is made of lead or other suitable material for shielding against radioactive emission from the generator. After the first milking" operation, there will be some eluant in the eluant conduit 27 from the shield to where the flexible tubing portion 29 of the eluant conduit is pinched between jaw members 183 and 169, but radiation from this amount of eluant is minor.

While, as above described, the elution is by use of an evacuated container 15 and suctioning of the eluant into the generator and the eluate out of the generator (i.e., a vacuum system), the principles of the invention are also applicable to a pressure system, as distinguished from a vacuum system, using a nonevacuated container or vial, and in which the eluant supply would be under pressure above atmospheric pressure or adapted for flow by gravity through the generator into the vial, and a vent would be provided in the stopper of the vial.

In view of the above, it will be seen that the several objects of the invention are achieved and other advantageous results attained.

As various changes could be made in the above constructions without departing from the scope of the invention, it is intended that all matter contained in the above description or shown in the accompanying drawings shall be interpreted as illustrative and not in a limiting sense.

What is claimed is:

1. Apparatus for eluting a daughter radioisotope from a parent radioisotope and for containerizing the resultant eluate in a container having a closure adapted to be pierced by a needle, said apparatus comprising:

a generator containing a supply of the parent radioisotope,

a shield enclosing the generator for shielding the user against radioactive emission from the generator,

means for holding a supply of eluant adjacent the shield and generator,

an eluant conduit extending from the eluant supply means through the shield and into the generator,

a tubular fitting adapted for attachment thereto at one end of a tubular needle for piercing said closure,

means adjacent the shield and generator mounting said tubular fitting for movement away from a retracted position in the direction of length of the needle to cause the needle to pierce said closure,

an eluate conduit extending from said generator through the shield and having a flexible tubing portion connected to the other end of said tubular fitting permitting movement of said fitting,

said eluant conduit, generator, eluate conduit and fitting constituting a closed passage from the eluant supply means to said needle,

and means associated with said fitting for effecting closure of said eluate conduit when said fitting is in its said retracted position and opening of said eluate conduit when said fitting is moved to cause the needle to pierce the closure of said container for flow of eluant from the eluant supply means through the eluant conduit into the generator for eluting the daughter radioisotope from the parent radioisotope in the generator and flow of the resultant eluate from the generator through the eluate conduit, fitting and needle into the container.

2. Apparatus as set forth in claim 1 wherein the means for efiecting closure of the eluate conduit comprises a member movable with the fitting for pinching closed the flexible tubing portion of the eluate conduit when the fitting is in its retracted position.

3. Apparatus as set forth in claim 2 having spring means for biasing the fitting toward its retracted position.

4. Apparatus as set forth in claim 1 wherein the mounting means for the fitting comprises a plunger and means guiding the plunger for vertical sliding movement downward from a raised retracted position toward a container positioned therebelow with its piercable closure at the top, the fitting being adapted for attachment thereto of the needle with the needle extending downward, the means for effecting closure of said eluate conduit comprising a jaw member on the plunger and a fixed jaw member thereabove, the flexible tubing portion of the eluate conduit extending between said jaw members and being pinched closed between said jaw members when the plunger is in its raised retracted position.

5. Apparatus as set forth in claim 4 having spring means biasing the plunger upward toward its raised retracted positron.

6. Apparatus as set forth in claim 5 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening.

7. Apparatus as set forth in claim 1 wherein the generator comprises an elongate closed vessel adapted for vertical disposition and having a convergent closed lower end, and means therein spaced from its lower end for maintaining the supply of the parent radioisotope spaced from its lower end, the eluant conduit being in communication with the upper end of the vessel and the eluate conduit being in communication with the lower end of the vessel.

8. Apparatus as set forth in claim 7 wherein the vessel comprises a tube having a hemispherical lower end and a stopper in it supper end, the means for maintaining the parent radioisotope spaced from its lower end comprising a filter mounted in the tube above its lower end, the parent radioisotope being confined between the filter and the stopper, the eluate conduit extending down through the stopper and terminating immediately below the stopper, the eluate conduit extending down through the stopper and the filter to the lower end of the tube.

9. Apparatus as set forth in claim 1 further comprising a case receiving the shield with the generator therein and also receiving the eluant supply means, said case being formed with a recess opening inward from the side of the case adapted to receive the container with its piercable closure at the top of the container and having a portion overhanging the recess, said fitting being carried at the lower end of a plunger vertically slidable in said overhanging portion of the case.

10. Apparatus as set forth in claim 9 wherein the means for effecting closure of the eluate conduit comprises a jaw member on the plunger adapted to pinch closed the flexible tubing portion of the eluate conduit against a portion of the case when the plunger is in a raised retracted position.

11. Apparatus as set forth in claim 10 having spring means for biasing the plunger upward to its retracted position.

12. Apparatus as set forth in claim 1 1 wherein the case comprises a bottom section and a cover, the bottom section having a bottom wall, means extending upward from the bottom defining a chamber for the shield, a peripheral wall extending upward from the bottom wall having a gap therein, a panel inset in the case at the gap defining said recess, and a head at the top of the recess, said plunger being vertically slidable in openings in the cover and said head and extending above the cover.

13. Apparatus as set forth in claim 12 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending within the case through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, said portion of the case being instituted by a jaw member on the inside of the cover at the said opening in the cover, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening against said jaw member on the inside of the cover.

14. Apparatus as set forth in claim 13 wherein said spring means comprises a coil compression spring surrounding the plunger reacting from said head against the jaw member on the plunger.

15. Apparatus as set forth in claim 12 wherein the cover is formed with at least one compartment for holding a supply of containers.

16. Apparatus as set forth in claim 1 for containerizing the eluate in an evacuated container having a closure adapted to be pierced by a needle, wherein the means for holding the supply of eluant holds it under atmospheric pressure and wherein, when the needle pierces said closure, the eluant is suctioned from the eluant supply means into the generator for eluting the daughter radioisotope from the parent radioisotope in the generator and the resultant eluate is suctioned from the generator through the eluate conduit, fitting and needle into the evacuated container.

17. Apparatus as set forth in claim 16 wherein the means for holding the supply of eluant under atmospheric pressure comprises a sealed plastic bag.

18. Apparatus as set forth in claim 16 wherein the means for effecting closure of the eluate conduit comprises a member movable with the fitting for pinching closed the flexible tubing portion of the eluate conduit when the fitting is in its retracted position.

19. Apparatus as set forth in claim 18 having spring means for biasing the fitting toward its retracted position.

20. Apparatus as set forth in claim 16 wherein the mounting means for the fitting comprises a plunger and means guiding the plunger for vertical sliding movement downward from a raised retracted position toward an evacuated container positioned therebelow with its piercable closure at the top, the

fitting being adapted for attachment thereto of the needle with the needle extending downward, the means for effecting closure of said eluate conduit comprising a jaw member on the plunger and a fixed jaw member thereabove, the flexible tubing portion of the eluate conduit extending between said jaw members and being pinched closed between said jaw members when the plunger is in its raised retracted position.

21. Apparatus as set forth in claim 20 having spring means biasing the plunger upward toward its raised retracted position.

22. Apparatus as set forth in claim 21 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening.

23. Apparatus as set forth in claim 16 wherein the generator comprises an elongate closed vessel adapted for vertical disposition and having a convergent closed lower end, and means therein spaced from its lower end for maintaining the supply of the parent radioisotope spaced from its lower end, the eluant conduit being in communication with the upper end of the vessel and the eluate conduit being in communication with the lower end of the vessel.

24. Apparatus as set forth in claim 23 wherein the vessel comprises a tube having a hemispherical lower end a stopper in its upper end, the means for maintaining the parent radioisotope spaced from its lower end comprising a filter mounted in the tube above its lower end, the parent radioisotope being confined between the filter and the stopper, the eluant conduit extending down through the stopper and terminating immediately below the stopper, the eluate conduit extending down through the stopper and the filter to the lower end of the tube.

25. Apparatus as set forth in claim 16 further comprising a case having a chamber receiving the shield with the generator therein, a compartment adjacent said chamber receiving the eluant supply means, said case being formed with a recess opening inward from the side of the case adapted to receive the evacuated container with its piercable closure at the top of the container and having a portion overhanging the recess, said fitting being carried at the lower end of a plunger vertically slidable in said overhanging portion of the case.

26. Apparatus as set forth in claim 25 wherein the means for effecting closure of the eluate conduit comprises a jaw member on the plunger adapted to pinch closed the flexible tubing portion of the eluate conduit against a portion of the case when the plunger is in a raised retracted position.

27. Apparatus as set forth in claim 26 having spring means for biasing the plunger upward to its retracted position.

28. Apparatus as set forth in claim 27 wherein the case comprises a bottom section and a cover, the bottom section having a bottom wall, means extending upward from the bottom defining said chamber for the shield, a peripheral wall extending upward from the bottom wall having a gap therein and a panel inset in the case at the gap defining said recess, and a head at the top of the recess, said plunger being vertically slidable in openings in the cover and said head and extending above the cover.

29. Apparatus as set forth in claim 28 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending within the case through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, said portion of the case being instituted by a jaw member on the inside of the cover at the said opening in the cover, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening against said jaw member on the inside of the cover.

30. pparatus as set forth in claim 29 wherein said spring means comprises a coil compression spring surrounding the plunger reacting from said head against the jaw member on the plunger.

31. Apparatus as set forth in claim 28 wherein the cover is formed with at least one compartment for holding a supply of evacuated containers. 

1. Apparatus for eluting a daughter radioisotope from a parent radioisotope and for containerizing the resultant eluate in a container having a closure adapted to be pierced by a needle, said apparatus comprising: a generator containing a supply of the parent radioisotope, a shield enclosing the generator for shielding the user against radioactive emission from the generator, means for holding a supply of eluant adjacent the shield and generator, an eluant conduit extending from the eluant supply means through the shield and into the generator, a tubular fitting adapted for attachment thereto at one end of a tubular needle for piercing said closure, means adjacent the shield and generator mounting said tubular fitting for movement away from a retracted position in the direction of length of the needle to cause the needle to pierce said closure, an eluate conduit extending from said generator through the shield and having a flexible tubing portion connected to the other end of said tubular fitting permitting movemEnt of said fitting, said eluant conduit, generator, eluate conduit and fitting constituting a closed passage from the eluant supply means to said needle, and means associated with said fitting for effecting closure of said eluate conduit when said fitting is in its said retracted position and opening of said eluate conduit when said fitting is moved to cause the needle to pierce the closure of said container for flow of eluant from the eluant supply means through the eluant conduit into the generator for eluting the daughter radioisotope from the parent radioisotope in the generator and flow of the resultant eluate from the generator through the eluate conduit, fitting and needle into the container.
 2. Apparatus as set forth in claim 1 wherein the means for effecting closure of the eluate conduit comprises a member movable with the fitting for pinching closed the flexible tubing portion of the eluate conduit when the fitting is in its retracted position.
 3. Apparatus as set forth in claim 2 having spring means for biasing the fitting toward its retracted position.
 4. Apparatus as set forth in claim 1 wherein the mounting means for the fitting comprises a plunger and means guiding the plunger for vertical sliding movement downward from a raised retracted position toward a container positioned therebelow with its piercable closure at the top, the fitting being adapted for attachment thereto of the needle with the needle extending downward, the means for effecting closure of said eluate conduit comprising a jaw member on the plunger and a fixed jaw member thereabove, the flexible tubing portion of the eluate conduit extending between said jaw members and being pinched closed between said jaw members when the plunger is in its raised retracted position.
 5. Apparatus as set forth in claim 4 having spring means biasing the plunger upward toward its raised retracted position.
 6. Apparatus as set forth in claim 5 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening.
 7. Apparatus as set forth in claim 1 wherein the generator comprises an elongate closed vessel adapted for vertical disposition and having a convergent closed lower end, and means therein spaced from its lower end for maintaining the supply of the parent radioisotope spaced from its lower end, the eluant conduit being in communication with the upper end of the vessel and the eluate conduit being in communication with the lower end of the vessel.
 8. Apparatus as set forth in claim 7 wherein the vessel comprises a tube having a hemispherical lower end and a stopper in it supper end, the means for maintaining the parent radioisotope spaced from its lower end comprising a filter mounted in the tube above its lower end, the parent radioisotope being confined between the filter and the stopper, the eluate conduit extending down through the stopper and terminating immediately below the stopper, the eluate conduit extending down through the stopper and the filter to the lower end of the tube.
 9. Apparatus as set forth in claim 1 further comprising a case receiving the shield with the generator therein and also receiving the eluant supply means, said case being formed with a recess opening inward from the side of the case adapted to receive the container with its piercable closure at the top of the container and having a portion overhanging the recess, said fitting being carried at the lower end of a plunger vertically slidable in said overhanging portion of the case.
 10. Apparatus as set forth in claim 9 wherein the means for effecting closure of the eluate conduit comprises a jaw member on the plunger adapted to pinch closed the flexible tubing portion of the eluate conduit against a portion of the case when the plunger is in a raised retracted position.
 11. Apparatus as set forth in claim 10 having spring means for biasing the plunger upward to its retracted position.
 12. Apparatus as set forth in claim 11 wherein the case comprises a bottom section and a cover, the bottom section having a bottom wall, means extending upward from the bottom defining a chamber for the shield, a peripheral wall extending upward from the bottom wall having a gap therein, a panel inset in the case at the gap defining said recess, and a head at the top of the recess, said plunger being vertically slidable in openings in the cover and said head and extending above the cover.
 13. Apparatus as set forth in claim 12 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending within the case through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, said portion of the case being instituted by a jaw member on the inside of the cover at the said opening in the cover, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening against said jaw member on the inside of the cover.
 14. Apparatus as set forth in claim 13 wherein said spring means comprises a coil compression spring surrounding the plunger reacting from said head against the jaw member on the plunger.
 15. Apparatus as set forth in claim 12 wherein the cover is formed with at least one compartment for holding a supply of containers.
 16. Apparatus as set forth in claim 1 for containerizing the eluate in an evacuated container having a closure adapted to be pierced by a needle, wherein the means for holding the supply of eluant holds it under atmospheric pressure and wherein, when the needle pierces said closure, the eluant is suctioned from the eluant supply means into the generator for eluting the daughter radioisotope from the parent radioisotope in the generator and the resultant eluate is suctioned from the generator through the eluate conduit, fitting and needle into the evacuated container.
 17. Apparatus as set forth in claim 16 wherein the means for holding the supply of eluant under atmospheric pressure comprises a sealed plastic bag.
 18. Apparatus as set forth in claim 16 wherein the means for effecting closure of the eluate conduit comprises a member movable with the fitting for pinching closed the flexible tubing portion of the eluate conduit when the fitting is in its retracted position.
 19. Apparatus as set forth in claim 18 having spring means for biasing the fitting toward its retracted position.
 20. Apparatus as set forth in claim 16 wherein the mounting means for the fitting comprises a plunger and means guiding the plunger for vertical sliding movement downward from a raised retracted position toward an evacuated container positioned therebelow with its piercable closure at the top, the fitting being adapted for attachment thereto of the needle with the needle extending downward, the means for effecting closure of said eluate conduit comprising a jaw member on the plunger and a fixed jaw member thereabove, the flexible tubing portion of the eluate conduit extending between said jaw members and being pinched closed between said jaw members when the plunger is in its raised retracted position.
 21. Apparatus as set forth in claim 20 having spring means biasing the plunger upward toward its raised retracted position.
 22. Apparatus as set forth in claim 21 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexiblE tubing portion of the eluate conduit extending through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening.
 23. Apparatus as set forth in claim 16 wherein the generator comprises an elongate closed vessel adapted for vertical disposition and having a convergent closed lower end, and means therein spaced from its lower end for maintaining the supply of the parent radioisotope spaced from its lower end, the eluant conduit being in communication with the upper end of the vessel and the eluate conduit being in communication with the lower end of the vessel.
 24. Apparatus as set forth in claim 23 wherein the vessel comprises a tube having a hemispherical lower end a stopper in its upper end, the means for maintaining the parent radioisotope spaced from its lower end comprising a filter mounted in the tube above its lower end, the parent radioisotope being confined between the filter and the stopper, the eluant conduit extending down through the stopper and terminating immediately below the stopper, the eluate conduit extending down through the stopper and the filter to the lower end of the tube.
 25. Apparatus as set forth in claim 16 further comprising a case having a chamber receiving the shield with the generator therein, a compartment adjacent said chamber receiving the eluant supply means, said case being formed with a recess opening inward from the side of the case adapted to receive the evacuated container with its piercable closure at the top of the container and having a portion overhanging the recess, said fitting being carried at the lower end of a plunger vertically slidable in said overhanging portion of the case.
 26. Apparatus as set forth in claim 25 wherein the means for effecting closure of the eluate conduit comprises a jaw member on the plunger adapted to pinch closed the flexible tubing portion of the eluate conduit against a portion of the case when the plunger is in a raised retracted position.
 27. Apparatus as set forth in claim 26 having spring means for biasing the plunger upward to its retracted position.
 28. Apparatus as set forth in claim 27 wherein the case comprises a bottom section and a cover, the bottom section having a bottom wall, means extending upward from the bottom defining said chamber for the shield, a peripheral wall extending upward from the bottom wall having a gap therein and a panel inset in the case at the gap defining said recess, and a head at the top of the recess, said plunger being vertically slidable in openings in the cover and said head and extending above the cover.
 29. Apparatus as set forth in claim 28 wherein the plunger is tubular, the fitting extending through the lower end of the plunger and adapted for attachment to its lower end of the needle, the flexible tubing portion of the eluate conduit extending within the case through a lateral opening in the plunger spaced from the lower end of the plunger and down through the plunger to a connection with the upper end of the fitting, said portion of the case being instituted by a jaw member on the inside of the cover at the said opening in the cover, the jaw member on the plunger being adapted to pinch closed said flexible tubing portion where it extends into said opening against said jaw member on the inside of the cover.
 30. Apparatus as set forth in claim 29 wherein said spring means comprises a coil compression spring surrounding the plunger reacting from said head against the jaw member on the plunger.
 31. Apparatus as set forth in claim 28 wherein the cover is formed with at least one compartment for holding a supply of evacuated containers. 